Spatiotemporal distribution and influencing factors of secondary organic aerosols in the summer atmosphere from the Bering Sea to the western North Pacific.

To better understand the formation process of biogenic and anthropogenic secondary organic aerosols (BSOA and ASOA) in the marine atmosphere under the background of global warming, aerosol samples were collected over three summers (i.e., 2014, 2016 and 2018) from the Bering Sea (BS) to the western North Pacific (WNP). The results showed that temporally, atmospheric concentrations of isoprene-derived SOA (SOAI) tracers were the lowest in 2014 regardless of the marine region, while atmospheric concentrations of monoterpenes-derived SOA (SOAM) tracers in this year were the highest and the aerosols were more aged than those in the other two years. In comparison, the concentrations of ß-caryophyllene-derived and toluene-derived SOA (SOAC and SOAA) tracers were relatively low overall. Spatially, the concentrations of SOA tracers were significantly higher over the WNP than over the BS, with SOA tracers over the BS mainly coming from marine sources, while the WNP was strongly influenced by terrestrial inputs. In particular, for land-influenced samples from the WNP, NOx-channel products of SOAI were more dependent on O3 and SO2 relative to HO2-channel product, and the high atmospheric oxidation capacity and SO2 could promote the formation of later-generation SOAM products. The extent of terrestrial influence was further quantified using a principal component analysis (PCA)-generalized additive model (GAM), which showed that terrestrial emissions explained more than half of the BSOA tracers' concentrations and contributed almost all of the ASOA tracer. In addition, the assessment of secondary organic carbon (SOC) highlighted the key role of anthropogenic activities in organic carbon levels in offshore areas. Our study revealed significant contributions of terrestrial natural and anthropogenic sources to different SOA over the WNP, and these relevant findings help improve knowledge about SOA in the marine atmosphere.

Molecular characteristics, sources and influencing factors of isoprene and monoterpenes secondary organic aerosol tracers in the marine atmosphere over the Arctic Ocean.

Biogenic secondary organic aerosols (BSOA) are important components of the remote marine atmosphere. However, the response of BSOA changes to sea ice reduction over the Arctic Ocean remains unclear. Here we investigated isoprene and monoterpenes secondary organic aerosol (SOAI and SOAM) tracers in three years of summer aerosol samples collected from the Arctic Ocean atmosphere. The results indicated that methyltetrols were the most abundant SOAI tracers, while the main oxidation products of monoterpenes varied over the years owing to different aerosol aging. The results of the principal component analysis (PCA)-generalized additive model (GAM) combined with correlation analysis suggested that SOAI tracers were mainly generated by the oxidation of isoprene from marine emissions, while SOAM tracers were probably more influenced by terrestrial transport. Estimation of secondary organic carbon (SOC) indicated that monoterpenes oxidation contributed more than isoprene and that sea ice changes had a relatively small effect on biogenic SOC concentration levels. Our study quantified the contribution of influencing factors to the atmospheric concentration of BSOA tracers in the Arctic Ocean, and showed that there were differences in the sources of precursors for different BSOA. Hence, our findings have contributed to a better understanding of the characteristics, sources and formation of SOA in the atmosphere of the Arctic Ocean.